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Hydrogen Peroxide Versus Hydrogen Generation at Bipolar Pd/Au Nano-catalysts Grown into an Intrinsically Microporous Polyamine (PIM-EA-TB)

Lina Wang, Mariolino Carta Orcid Logo, Richard Malpass-Evans, Neil B. McKeown, Philip J. Fletcher, Diana Lednitzky, Frank Marken

Electrocatalysis, Volume: 12, Issue: 6, Pages: 771 - 784

Swansea University Author: Mariolino Carta Orcid Logo

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DOI (Published version): 10.1007/s12678-021-00692-5

Abstract

Binding of PdCl42− into the polymer of intrinsic microporosity PIM-EA-TB (on a Nylon mesh substrate) followed by borohydride reduction leads to uncapped Pd(0) nano-catalysts with typically 3.2 ± 0.2 nm diameter embedded within the microporous polymer host structure. Spontaneous reaction of Pd(0) wit...

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Published in: Electrocatalysis
ISSN: 1868-2529 1868-5994
Published: Springer Science and Business Media LLC 2021
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URI: https://cronfa.swan.ac.uk/Record/cronfa58668
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spelling 2021-11-30T17:09:45.6811950 v2 58668 2021-11-15 Hydrogen Peroxide Versus Hydrogen Generation at Bipolar Pd/Au Nano-catalysts Grown into an Intrinsically Microporous Polyamine (PIM-EA-TB) 56aebf2bba457f395149bbecbfa6d3eb 0000-0003-0718-6971 Mariolino Carta Mariolino Carta true false 2021-11-15 CHEM Binding of PdCl42− into the polymer of intrinsic microporosity PIM-EA-TB (on a Nylon mesh substrate) followed by borohydride reduction leads to uncapped Pd(0) nano-catalysts with typically 3.2 ± 0.2 nm diameter embedded within the microporous polymer host structure. Spontaneous reaction of Pd(0) with formic acid and oxygen is shown to result in the competing formation of (i) hydrogen peroxide (at low formic acid concentration in air; with optimum H2O2 yield at 2 mM HCOOH), (ii) water, or (iii) hydrogen (at higher formic acid concentration or under argon). Next, a spontaneous electroless gold deposition process is employed to attach gold (typically 10- to 35-nm diameter) to the nano-palladium in PIM-EA-TB to give an order of magnitude enhanced production of H2O2 with high yields even at higher HCOOH concentration (suppressing hydrogen evolution). Pd and Au work hand-in-hand as bipolar electrocatalysts. A Clark probe method is developed to assess the catalyst efficiency (based on competing oxygen removal and hydrogen production) and a mass spectrometry method is developed to monitor/optimise the rate of production of hydrogen peroxide. Heterogenised Pd/Au@PIM-EA-TB catalysts are effective and allow easy catalyst recovery and reuse for hydrogen peroxide production. Journal Article Electrocatalysis 12 6 771 784 Springer Science and Business Media LLC 1868-2529 1868-5994 Biomass; Disinfection; Heterogenised palladium; Epoxidation; Hydrogen 1 11 2021 2021-11-01 10.1007/s12678-021-00692-5 COLLEGE NANME Chemistry COLLEGE CODE CHEM Swansea University China Scholarship Council (201906870022); EP/K004956/1 from the EPSRC 2021-11-30T17:09:45.6811950 2021-11-15T11:27:42.8997098 Faculty of Science and Engineering School of Engineering and Applied Sciences - Chemistry Lina Wang 1 Mariolino Carta 0000-0003-0718-6971 2 Richard Malpass-Evans 3 Neil B. McKeown 4 Philip J. Fletcher 5 Diana Lednitzky 6 Frank Marken 7 58668__21742__676a8cac88c349b59cb673e620cf3a03.pdf 58668.pdf 2021-11-30T17:07:41.7309899 Output 5197301 application/pdf Version of Record true © The Author(s) 2021. This article is licensed under a Creative Commons Attribution 4.0 International License true eng http://creativecommons.org/licenses/by/4.0/
title Hydrogen Peroxide Versus Hydrogen Generation at Bipolar Pd/Au Nano-catalysts Grown into an Intrinsically Microporous Polyamine (PIM-EA-TB)
spellingShingle Hydrogen Peroxide Versus Hydrogen Generation at Bipolar Pd/Au Nano-catalysts Grown into an Intrinsically Microporous Polyamine (PIM-EA-TB)
Mariolino Carta
title_short Hydrogen Peroxide Versus Hydrogen Generation at Bipolar Pd/Au Nano-catalysts Grown into an Intrinsically Microporous Polyamine (PIM-EA-TB)
title_full Hydrogen Peroxide Versus Hydrogen Generation at Bipolar Pd/Au Nano-catalysts Grown into an Intrinsically Microporous Polyamine (PIM-EA-TB)
title_fullStr Hydrogen Peroxide Versus Hydrogen Generation at Bipolar Pd/Au Nano-catalysts Grown into an Intrinsically Microporous Polyamine (PIM-EA-TB)
title_full_unstemmed Hydrogen Peroxide Versus Hydrogen Generation at Bipolar Pd/Au Nano-catalysts Grown into an Intrinsically Microporous Polyamine (PIM-EA-TB)
title_sort Hydrogen Peroxide Versus Hydrogen Generation at Bipolar Pd/Au Nano-catalysts Grown into an Intrinsically Microporous Polyamine (PIM-EA-TB)
author_id_str_mv 56aebf2bba457f395149bbecbfa6d3eb
author_id_fullname_str_mv 56aebf2bba457f395149bbecbfa6d3eb_***_Mariolino Carta
author Mariolino Carta
author2 Lina Wang
Mariolino Carta
Richard Malpass-Evans
Neil B. McKeown
Philip J. Fletcher
Diana Lednitzky
Frank Marken
format Journal article
container_title Electrocatalysis
container_volume 12
container_issue 6
container_start_page 771
publishDate 2021
institution Swansea University
issn 1868-2529
1868-5994
doi_str_mv 10.1007/s12678-021-00692-5
publisher Springer Science and Business Media LLC
college_str Faculty of Science and Engineering
hierarchytype
hierarchy_top_id facultyofscienceandengineering
hierarchy_top_title Faculty of Science and Engineering
hierarchy_parent_id facultyofscienceandengineering
hierarchy_parent_title Faculty of Science and Engineering
department_str School of Engineering and Applied Sciences - Chemistry{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Chemistry
document_store_str 1
active_str 0
description Binding of PdCl42− into the polymer of intrinsic microporosity PIM-EA-TB (on a Nylon mesh substrate) followed by borohydride reduction leads to uncapped Pd(0) nano-catalysts with typically 3.2 ± 0.2 nm diameter embedded within the microporous polymer host structure. Spontaneous reaction of Pd(0) with formic acid and oxygen is shown to result in the competing formation of (i) hydrogen peroxide (at low formic acid concentration in air; with optimum H2O2 yield at 2 mM HCOOH), (ii) water, or (iii) hydrogen (at higher formic acid concentration or under argon). Next, a spontaneous electroless gold deposition process is employed to attach gold (typically 10- to 35-nm diameter) to the nano-palladium in PIM-EA-TB to give an order of magnitude enhanced production of H2O2 with high yields even at higher HCOOH concentration (suppressing hydrogen evolution). Pd and Au work hand-in-hand as bipolar electrocatalysts. A Clark probe method is developed to assess the catalyst efficiency (based on competing oxygen removal and hydrogen production) and a mass spectrometry method is developed to monitor/optimise the rate of production of hydrogen peroxide. Heterogenised Pd/Au@PIM-EA-TB catalysts are effective and allow easy catalyst recovery and reuse for hydrogen peroxide production.
published_date 2021-11-01T04:15:22Z
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